scholarly journals Towards a better understanding of the origins, chemical composition and aging of oxygenated organic aerosols: case study of a Mediterranean industrialized environment, Marseille

2013 ◽  
Vol 13 (15) ◽  
pp. 7875-7894 ◽  
Author(s):  
I. El Haddad ◽  
B. D'Anna ◽  
B. Temime-Roussel ◽  
M. Nicolas ◽  
A. Boreave ◽  
...  

Abstract. As part of the FORMES summer 2008 experiment, an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) was deployed at an urban background site in Marseille to investigate the sources and aging of organic aerosols (OA). France's second largest city and the largest port in the Mediterranean, Marseille, provides a locale that is influenced by significant urban industrialized emissions and an active photochemistry with very high ozone concentrations. Particle mass spectra were analyzed by positive matrix factorization (PMF2) and the results were in very good agreement with previous apportionments obtained using a chemical mass balance (CMB) approach coupled to organic markers and metals (El Haddad et al., 2011a). AMS/PMF2 was able to identify for the first time, to the best of our knowledge, the organic aerosol emitted by industrial processes. Even with significant industries in the region, industrial OA was estimated to contribute only ~ 5% of the total OA mass. Both source apportionment techniques suggest that oxygenated OA (OOA) constitutes the major fraction, contributing ~ 80% of OA mass. A novel approach combining AMS/PMF2 data with 14C measurements was applied to identify and quantify the fossil and non-fossil precursors of this fraction and to explicitly assess the related uncertainties. Results show with high statistical confidence that, despite extensive urban and industrial emissions, OOA is overwhelmingly non-fossil, formed via the oxidation of biogenic precursors, including monoterpenes. AMS/PMF2 results strongly suggest that the variability observed in the OOA chemical composition is mainly driven in our case by the aerosol photochemical age. This paper presents the impact of photochemistry on the increase of OOA oxygenation levels, formation of humic-like substances (HULIS) and the evolution of α-pinene SOA (secondary OA) components.

2022 ◽  
Author(s):  
Victor Chaplygin ◽  
Tatiana Minkina ◽  
Saglara Mandzhieva ◽  
Dina Nevidomskaya ◽  
Natalia Chernikova ◽  
...  

Over the pastdecade, particular attention has been paid to studies of the chemical composition of medical plants to identify the possible negative consequences of using raw plant material polluted with heavy metals for the production of medical drugs. In our study, we analyzed the chemical composition of the medical plants growing in the impact area of the Novocherkassk power station. Specifically, the plants Artemisia austriaca, Poa pratensis and Elytrigia repenswere examined for the analysis.The content and distribution of Zn and Cd, which are most distributed in industrial emissions and belong to the first class of hazardous elements, were measured. The maximum permissible content (MPC) of Zn in the raw material of Artemisia austriaca and Elytrigia repens was found, as was the maximum content of Cd in all analyzed plants growing in the 5km area around thepower station. The plant Artemisia austriacawasfound to have Zn and Cd accumulation in itsabovegroundcomponents, while in Poa pratensis and Elytrigia repens, accumulation was in the roots. The morphobiometric parameters of the plants were mostly dependent on the soil properties, followed by the degree of technogenic load. The content of Zn and Cd in the medical drugs was higher than the MPC without visible features of heavy metal pollution and so these plants weredangerous for human health. Keywords: heavy metals, technogenic load, phytoreagents, morphometric parameters


2016 ◽  
Vol 16 (4) ◽  
pp. 2631-2640 ◽  
Author(s):  
Guohua Zhang ◽  
Xinhui Bi ◽  
Ning Qiu ◽  
Bingxue Han ◽  
Qinhao Lin ◽  
...  

Abstract. Knowledge on the microphysical properties of atmospheric aerosols is essential to better evaluate their radiative forcing. This paper presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in Guangzhou, China. Vacuum aerodynamic diameter, chemical compositions, and light-scattering intensities of individual particles were simultaneously measured by a single-particle aerosol mass spectrometer (SPAMS) during the fall of 2012. On the basis of Mie theory, n at a wavelength of 532 nm and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and Metal-rich. The results indicate the presence of spherical or nearly spherical shapes for the majority of particle types, whose partial scattering cross-section versus sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47–1.53), majority of particle types exhibited a wide range of ρeff (0.87–1.51 g cm−3). The OC group is associated with the lowest ρeff (0.87–1.07 g cm−3), and the Metal-rich group with the highest ones (1.29–1.51 g cm−3). It is noteworthy that a specific EC type exhibits a complex scattering curve versus size due to the presence of both compact and irregularly shaped particles. Overall, the results on the detailed relationship between physical and chemical properties benefits future research on the impact of aerosols on visibility and climate.


2020 ◽  
Author(s):  
Najin Kim ◽  
Seong Soo Yum ◽  
Minsu Park ◽  
Jong Sung Park ◽  
Hye Jung Shin ◽  
...  

Abstract. Chemical effects on the size-resolved hygroscopicity of urban aerosols were examined based on the KORUS-AQ field campaign data. The information on size-resolved hygroscopicity and chemical composition of aerosols were obtained by a hygroscopic tandem differential mobility analyzer (HTDMA) and a high-resolution time of flight aerosol mass spectrometer (HR-ToF-AMS), respectively. Good correspondences were shown between the measured and estimated κ values calculated from the combination of bulk chemical composition data and oxidation parameters of organic aerosols (f44 and O/C). These results infer that chemical composition is closely associated with aerosol hygroscopicity. However, the correlation between measured and estimated κ values degraded as particle size decreased, implying that the size-resolved chemical composition data is required for more detailed hygroscopicity analysis. In addition to size-resolved chemical data, the m/z tracer method was applied for size-resolved organic factors. Specifically, m/z 57 and 44 were used as AMS spectral markers for HOA and OOA, respectively. These size-resolved chemical composition data were found to be critical in explaining the size-dependent hygroscopicity as well as the diurnal variation of κ for small particles, i.e., low κ in the morning and high κ in the afternoon. Additionally, aerosol mixing state information was associated with the size-resolved chemical composition data. That is, the relationship between the number fraction of each hygroscopicity mode and the volume fraction of different chemical composition was investigated. It was found that the HOA volume fraction explained about 60 % of the variation of less hygroscopic (LH) mode number fraction for externally mixed aerosols.


2018 ◽  
Author(s):  
Liqing Hao ◽  
Olga Garmash ◽  
Mikael Ehn ◽  
Pasi Miettinen ◽  
Paola Massoli ◽  
...  

Abstract. Characterizing aerosol chemical composition in response to meteorological changes and atmospheric chemistry is important to gain insights into new particle formation mechanisms. A BAECC (Biogenic Aerosols-Effects on Clouds and Climate) campaign was conducted during the spring 2014 at SMEAR II station (Station for Measuring Forest Ecosystem-Aerosol Relations) in Finland. The particles were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). A PBL (planetary boundary layer) dilution model was developed to assist interpreting the measurement results. Right before nucleation events, the mass concentrations of organic and sulfate aerosol species were both decreased rapidly along with the growth of PBL heights. However, the mass fraction of sulfate aerosol of the total aerosol mass was increased, in contrast to a decrease for the organic mass fraction. Meanwhile, an increase of LVOOA (low-volatility oxygenated organic aerosol) mass fraction of the total organic mass was observed, in distinct comparison to a reduction of SVOOA (semi-volatile OOA) mass fraction. Our results demonstrate that, at the beginning of nucleation events, the observed sulfate aerosol mass was mainly driven by vertical turbulent mixing of sulfate-rich aerosols between the residual layer and the newly formed boundary layer, while the condensation of sulfuric acid played a minor role in interpreting the measured sulfate mass concentration. For the measured organic aerosols, their temporal profiles were mainly driven by dilution from PBL development, organic aerosol mixing in different boundary layers and/or condensation of organic vapors, but accurate measurements of organic vapor concentrations and characterization on the spatial aerosol chemical composition are required. In general, the observed aerosol particles by AMS are subjected to joint effects of PBL dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During aerosol growth periods in the night time, the mass concentrations of organic aerosols and organic nitrate aerosols were both increased. The increase of SVOOA mass correlated well with the calculated increase of condensed HOMs (highly oxygenated organic molecules) mass. To our knowledge, our results are the first atmospheric observations showing a connection between increase in SVOOA and condensed HOMs during the night time.


2015 ◽  
Vol 32 (6) ◽  
pp. 877-888 ◽  
Author(s):  
Junke Zhang ◽  
Yuesi Wang ◽  
Xiaojuan Huang ◽  
Zirui Liu ◽  
Dongsheng Ji ◽  
...  

2012 ◽  
Vol 12 (4) ◽  
pp. 2215-2227 ◽  
Author(s):  
Y. L. Sun ◽  
Q. Zhang ◽  
J. J. Schwab ◽  
W.-N. Chen ◽  
M.-S. Bae ◽  
...  

Abstract. Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML), equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE) – a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1) species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz) of gaseous pollutants (e.g. HCHO, NO2, NO, O3, and CO2, etc.), black carbon (BC), and particle number concentrations and size distributions. Particulate organics varied dramatically during periods with high traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA), a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate) and oxygenated OA (OOA) showed much smoother variations indicating minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60%) with HOA accounting for a major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ∼120 nm and 500 nm (vacuum aerodynamic diameter, Dva), respectively. OOA and inorganic species appear to be internally mixed in the accumulation mode peaking at ∼500–600 nm. The enhancement of organics in traffic emissions mainly occurred at ultrafine mode dominated by HOA, with little relation to the OOA-dominated accumulation mode. From Fast Mobility Particle Sizer (FMPS) measurements, a large increase in number concentration at ∼10 nm (mobility number mean diameter, Dm) was also found due to traffic influence; though these particles typically contribute a minor fraction of total particle mass. The observed rapid variations of aerosol chemistry and microphysics may have significant implications for near-highway air pollution characterization and exposure assessments.


Author(s):  
L. Zhao ◽  
C. Yang

Abstract. The chemical composition of aerosols was investigated using regular environmental air quality observation, a single particle aerosol mass spectrometer (SPAMS 0515) and an ambient ion monitor (URG 9000D) in Xiamen in 2018. The results showed that the annual average mass concentrations of PM2.5 was 22 μm/m3, and concentrations of water-soluble inorganic ions was 9.94 μm/m3 which accounted for 45.2% of PM2.5. SO42−, NO3− and NH4+ were main components of secondary reactions which contributed more than 77 percent of water-soluble inorganic ion concentration. As a coastal city, Cl− and Na+ contributed 13.9 percent of water-soluble inorganic ion concentration. Based on single particle aerosol mass spectrometer analysing, mobile sources emission was the most important sources of particle matter which contributed over 30%.


2012 ◽  
Vol 12 (2) ◽  
pp. 4831-4866
Author(s):  
M. Elsasser ◽  
M. Crippa ◽  
J. Orasche ◽  
P. F. DeCarlo ◽  
M. Oster ◽  
...  

Abstract. The impact of wood combustion on ambient aerosols was investigated in Augsburg, Germany during a winter measurement campaign of a six-week period. Special attention was paid to the high time resolution observations of wood combustion with different mass spectrometric methods. Here we present and compare the results from an Aerodyne aerosol mass spectrometer (AMS) and gas chromatographic – mass spectrometric (GC-MS) analysed PM1 filters on an hourly basis. This includes source apportionment of the AMS derived organic mass by using positive matrix factorisation (PMF) and analysis of levoglucosan as wood combustion marker, respectively. In the measurement period nitrate and organics are the main contributors to the defined submicron particle mass with 28% and 35%, respectively. To the latter wood combustion organic aerosol (WCOA) contributes 23% on average and 27% in the evening and night-time. Conclusively, wood combustion has a strong influence on the organics and overall aerosol composition. Levoglucosan accounts for 14% of WCOA mass with a higher percentage in comparison to other studies. The ratio between the mass of levoglucosan and organic carbon amounts to 0.06. This study is unique in the one-hour time resolution comparison between the wood combustion results of the AMS and the GC-MS analysed filter method at a PM1 particle size range. This comparison of the concentration courses of the PMF WCOA factor, levoglucosan estimated by the AMS data and the levoglucosan measured by GC-MS is highly correlated, and a detailed discussion on the contributors to the wood combustion marker ion at mass-to-charge ratio 60 will be given. This offers a suitable application possibility for the description of the wood combustion course by the WCOA factor and the levoglucosan concentration estimated by AMS data. However, quantitative description of the levoglucosan concentration estimated by the AMS data is difficult due to the offset of latter compared to measured levoglucosan by the GC-MS.


2015 ◽  
Vol 15 (23) ◽  
pp. 13569-13584 ◽  
Author(s):  
Y. Liu ◽  
J. Liggio ◽  
R. Staebler ◽  
S.-M. Li

Abstract. As a class of brown carbon, organonitrogen compounds originating from the heterogeneous uptake of NH3 by secondary organic aerosol (SOA) have received significant attention recently. In the current work, particulate organonitrogen formation during the ozonolysis of α-pinene and the OH oxidation of m-xylene in the presence of ammonia (34–125 ppb) was studied in a smog chamber equipped with a high resolution time-of-flight aerosol mass spectrometer and a quantum cascade laser instrument. A large diversity of nitrogen-containing organic (NOC) fragments was observed which were consistent with the reactions between ammonia and carbonyl-containing SOA. Ammonia uptake coefficients onto SOA which led to organonitrogen compounds were reported for the first time, and were in the range of ∼ 10-3–10−2, decreasing significantly to < 10-5 after 6 h of reaction. At the end of experiments (~ 6 h) the NOC mass contributed 8.9 ± 1.7 and 31.5 ± 4.4 wt % to the total α-pinene- and m-xylene-derived SOA, respectively, and 4–15 wt % of the total nitrogen in the system. Uptake coefficients were also found to be positively correlated with particle acidity and negatively correlated with NH3 concentration, indicating that heterogeneous reactions were responsible for the observed NOC mass, possibly limited by liquid phase diffusion. Under these conditions, the data also indicate that the formation of NOC can compete kinetically with inorganic acid neutralization. The formation of NOC in this study suggests that a significant portion of the ambient particle associated N may be derived from NH3 heterogeneous reactions with SOA. NOC from such a mechanism may be an important and unaccounted for source of PM associated nitrogen. This mechanism may also contribute to the medium or long-range transport and wet/dry deposition of atmospheric nitrogen.


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